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The coordination of tBuNC and CO with the diarsenido complexes (C5Me5)2An(η2‐As2Mes2), An=Th, U, has been investigated. For the first time, a comparison between isostructural complexes of ThIV and UIV has been possible with CO; density functional calculations indicated an appreciable amount of π backbonding that originates from charge transfer from an actinide‐arsenic sigma bond. The calculated CO...